Currently, one of the challenges in high-resolution transmission electron microscopy (TEM) studies of nanomaterials is to make contamination-free materials in a simple and time-efficient way. Here, a method is demonstrated that combines nanosecond-pulsed laser dewetting of thin films with a film float-off technique to realize nanostructures (NSs) on electron-transparent substrates in a robust and rapid manner. NSs of metal (Ag) and bimetals (AgCo, AuCo) ranging from 20 to 150 nm are synthesized on thin carbon film deposited on mica substrates. The NS/carbon system is subsequently transferred onto TEM grids by a float-off process resulting from debonding of the carbon from mica due to their contrasting hydrophobic nature. This process enables the fabrication of different NSs on flexible and electron-transparent substrates.